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Title: Enabling Structure/Interface Regulation for High Performance Ni-Rich Cathodes

Journal Article · · Advanced Functional Materials

Here, further commercialization of Ni-rich layered cathodes is hindered by severe structure/interface degradation and kinetic hindrance that occur during electrochemical operation, which leads to safety risks and reduced range in electric vehicles (EVs). Herein, by selecting elements with different solubility properties, a multifunctional strategy that synchronously fabricates perovskite-type SrZrO3 coating and Sr/Zr co-doping is employed to strengthen the structure/interface stability and the Li+ transport mobility of LiNi0.85Co0.10Mn0.05O2 (NCM). Perovskite-type SrZrO3 protective layers formed on the particle surface can substantially mitigate the unexpected interfacial side reactions and surface phase transitions. In addition, a robust crystal framework is constructed by optimizing local O coordination through the introduction of strong Zr-O bonds. Notably, Li+ diffusion kinetics is effectively improved due to expanded cell parameters and O-Li-O slab spacing with the incorporation of large-diameter Sr pillar ions, as revealed by X-ray diffraction. As a result, the Sr/Zr-modified NCM achieves a remarkable capacity retention of 99.4% after 200 cycles at 1 C, and a high rate capacity of 168.9 mAh g-1 at 10 C. This work opens new avenues to develop high-performance NCM cathodes with high energy and high power for EVs with long calendar life.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
National Natural Science Foundation of China (NSFC); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
2371815
Journal Information:
Advanced Functional Materials, Journal Name: Advanced Functional Materials Journal Issue: 51 Vol. 33; ISSN 1616-301X
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

References (53)

High‐Voltage Charging‐Induced Strain, Heterogeneity, and Micro‐Cracks in Secondary Particles of a Nickel‐Rich Layered Cathode Material journal March 2019
New Insight into Microstructure Engineering of Ni‐Rich Layered Oxide Cathode for High Performance Lithium Ion Batteries journal February 2021
Review on the Binders for Sustainable High‐Energy‐Density Lithium Ion Batteries: Status, Solutions, and Prospects journal July 2023
Elucidating and Mitigating High‐Voltage Degradation Cascades in Cobalt‐Free LiNiO 2 Lithium‐Ion Battery Cathodes journal November 2021
A Comprehensive Analysis of the Interphasial and Structural Evolution over Long‐Term Cycling of Ultrahigh‐Nickel Cathodes in Lithium‐Ion Batteries journal October 2019
Polycrystalline and Single Crystalline NCM Cathode Materials—Quantifying Particle Cracking, Active Surface Area, and Lithium Diffusion journal March 2021
Hard Carbon Anodes for Next‐Generation Li‐Ion Batteries: Review and Perspective journal September 2021
Atomical Reconstruction and Cationic Reordering for Nickel‐Rich Layered Cathodes journal January 2022
Challenges and Strategies towards Single‐Crystalline Ni‐Rich Layered Cathodes journal July 2022
Kinetic Limitations in Single‐Crystal High‐Nickel Cathodes journal November 2020
Mg‐Pillared LiCoO 2 : Towards Stable Cycling at 4.6 V journal January 2021
Competitive Doping Chemistry for Nickel‐Rich Layered Oxide Cathode Materials journal March 2022
Roles of Fast‐Ion Conductor LiTaO3 Modifying Ni‐rich Cathode Material for Li‐Ion Batteries journal March 2021
Crack-free single-crystalline Co-free Ni-rich LiNi0.95Mn0.05O2 layered cathode journal January 2022
Electronic structural changes of the electrochemically Li-ion deintercalated LiNi0.8Co0.15Al0.05O2 cathode material investigated by X-ray absorption spectroscopy journal December 2007
Effect of Mg doping on the local structure of LiMgyCo1−yO2 cathode material investigated by X-ray absorption spectroscopy journal April 2014
Thermal stress-induced charge and structure heterogeneity in emerging cathode materials journal May 2020
Fundamental and solutions of microcrack in Ni-rich layered oxide cathode materials of lithium-ion batteries journal May 2021
Chemical-Mechanical Effects in Ni-Rich Cathode Materials journal February 2022
Impact of Microcrack Generation and Surface Degradation on a Nickel-Rich Layered Li[Ni 0.9 Co 0.05 Mn 0.05 ]O 2 Cathode for Lithium-Ion Batteries journal September 2017
A Mg-Doped High-Nickel Layered Oxide Cathode Enabling Safer, High-Energy-Density Li-Ion Batteries journal January 2019
Oxygen K-edge X-ray Absorption Spectra journal April 2020
Charge-Transfer-Induced Lattice Collapse in Ni-Rich NCM Cathode Materials during Delithiation journal October 2017
Intergranular Cracking as a Major Cause of Long-Term Capacity Fading of Layered Cathodes journal May 2017
Electrochemical Performance and Elevated Temperature Properties of the TiO2-Coated Li[Ni0.8Co0.1Mn0.1]O2 Cathode Material for High-Safety Li-Ion Batteries journal May 2021
Capacity Fading Mechanisms in Ni-Rich Single-Crystal NCM Cathodes journal July 2021
Self-Passivation of a LiNiO 2 Cathode for a Lithium-Ion Battery through Zr Doping journal June 2018
Structural and Electrochemical Aspects of LiNi 0.8 Co 0.1 Mn 0.1 O 2 Cathode Materials Doped by Various Cations journal January 2019
Unraveling the Cationic and Anionic Redox Reactions in a Conventional Layered Oxide Cathode journal October 2019
Multiscale Crystal Field Effect for High-Performance Ultrahigh-Ni Layered Cathode journal June 2023
Understanding Li Diffusion in Li-Intercalation Compounds journal May 2012
Redox Chemistry and the Role of Trapped Molecular O2 in Li-Rich Disordered Rocksalt Oxyfluoride Cathodes journal December 2020
Intrinsic Kinetic Limitations in Substituted Lithium-Layered Transition-Metal Oxide Electrodes journal March 2020
Hierarchical nickel valence gradient stabilizes high-nickel content layered cathode materials journal April 2021
Surface enrichment and diffusion enabling gradient-doping and coating of Ni-rich cathode toward Li-ion batteries journal July 2021
In situ inorganic conductive network formation in high-voltage single-crystal Ni-rich cathodes journal September 2021
Transition metal-doped Ni-rich layered cathode materials for durable Li-ion batteries journal November 2021
Approaching the capacity limit of lithium cobalt oxide in lithium ion batteries via lanthanum and aluminium doping journal June 2018
High-nickel layered oxide cathodes for lithium-based automotive batteries journal January 2020
Understanding Co roles towards developing Co-free Ni-rich cathodes for rechargeable batteries journal February 2021
Reactive boride infusion stabilizes Ni-rich cathodes for lithium-ion batteries journal March 2021
Layered Li–Ni–Mn–Co oxide cathodes journal September 2021
Introducing high-valence elements into cobalt-free layered cathodes for practical lithium-ion batteries journal September 2022
Bulk fatigue induced by surface reconstruction in layered Ni-rich cathodes for Li-ion batteries journal August 2020
Resolving complex intralayer transition motifs in high-Ni-content layered cathode materials for lithium-ion batteries journal January 2023
Compositionally complex doping for zero-strain zero-cobalt layered cathodes journal September 2022
Revealing the role of NH 4 VO 3 treatment in Ni-rich cathode materials with improved electrochemical performance for rechargeable lithium-ion batteries journal January 2018
Stabilizing nickel-rich layered oxide cathodes by magnesium doping for rechargeable lithium-ion batteries journal January 2019
Overall structural modification of a layered Ni-rich cathode for enhanced cycling stability and rate capability at high voltage journal January 2019
Suppressing detrimental phase transitions via tungsten doping of LiNiO 2 cathode for next-generation lithium-ion batteries journal January 2019
Electrodes with High Power and High Capacity for Rechargeable Lithium Batteries journal February 2006
On The Efficacy of Cobalt Boride Coating on NMC-811 Cathode Under Vinylene Carbonate Additive, High Temperature and Air Shelving Conditions journal January 2023
Dependence of Cell Failure on Cut-Off Voltage Ranges and Observation of Kinetic Hindrance in LiNi 0.8 Co 0.15 Al 0.05 O 2 journal January 2018